BACKGROUND Membrane technology has attracted increasing interest in the field of separation and purification. Unfortunately, conventional membrane materials are usually derived from non‐renewable fossil resources that are difficult to degrade at the end of their life. In this work, as a sustainable alternative to the conventional polymer membrane, the biobased ploy (L‐lactic acid) (PLLA) hybrid membrane was successfully fabricated through the incorporation of modified natural halloysite nanotubes (HNTs). RESULTS The PLLA/HNT hybrid membranes were analysed by attenuated total reflectance‐Fourier transform infrared spectroscopy (ATR‐FTIR), X‐ray diffraction (XRD), scanning electron microscopy (SEM), X‐ray diffraction (XRD), and contact angle measurement. The pure water flux of the hybrid membrane increased from 140.3 to 329.7 L.m−3.h−1, while the bovine serum albumin (BSA) rejection ratio decreased from 94.3 to 82.7% with increasing HNT loading content from 0 to 1 wt%. Moreover, the addition of HNTs could also enhance the antifouling performance of the hybrid membrane. CONCLUSION The green PLLA/HNT hybrid membrane was successfully made from the recoverable and biodegradable PLLA and naturally occurring HNTs. Compared with the PLLA‐based membranes reported in the literature, the PLLA/HNT hybrid membranes presented relatively high permeability, moderate BSA rejection, and good antifouling performance. The green poly (L‐lactic acid) hybrid membranes hold great promise for practical application as they can contribute to a circular economy and sustainable development. © 2022 Society of Chemical Industry (SCI).